JH

Organic Intermediates and Reaction Transformations

Organic Intermediates and Reaction Transformations

Organic Intermediates

  • Most organic reactions proceed via a reactive, short-lived intermediate species.

  • These intermediates typically have a carbon atom with a valency of 2 or 3.

  • Examples include carbocations, carbanions, free radicals, carbenes, and nitrenes.

  • Carbanions are unique among these intermediates as they possess a complete octet around the carbon atom.

  • Nitrenes are nitrogen analogs of carbenes, featuring charges and unpaired electrons on nitrogen atoms.

Carbocations

  • Carbocations are organic species with a positively charged carbon atom bonded to only six electrons.

  • The positively charged carbon is \text{sp}^2 hybridized.

  • The three sp^2 hybridized orbitals form bonds with three substituents, resulting in a planar configuration with bond angles of 120^o to minimize electron pair repulsion.

  • An empty p orbital is perpendicular to this plane.

  • Carbocations are highly reactive due to their electron deficiency.

Classification of Carbocations
  • Carbocations are classified as primary (1^o), secondary (2^o), or tertiary (3^o) based on the number of carbon atoms directly attached to the positively charged carbon.

Factors Affecting Carbocation Stability
  • Several factors influence carbocation stability:

    • Inductive effect

    • Hyperconjugative effect

    • Resonance effect

    • Steric effect

    • Aromatic system formation

Inductive Effect
  • Charge-dispersing factors stabilize ions.

  • Alkyl groups exert a +I (electron-releasing inductive) effect, partially neutralizing the positive charge on the carbocation.

  • This charge dispersion leads to stabilization.

  • Carbocation stability increases with the number of alkyl groups attached; for example, methyl groups in isopropyl cation stabilize the system through their +I effects.

Hyperconjugative Effect
  • Alkyl groups can reduce the positive charge via hyperconjugation.

  • The positive charge is dispersed over the α-hydrogens, stabilizing the system.

  • The stability of methyl-substituted carbocations increases with the number of α-hydrogens (hyperconjugative forms).

Resonance Effect
  • Resonance is a significant stabilizing factor.

  • Effective charge delocalization occurs when the positive carbon is adjacent to a double bond, leading to stabilization.

  • Allyl and benzyl cations are highly stabilized by resonance.

Steric Effect
  • Steric effects can enhance the stability of tertiary carbocations with bulky alkyl groups.

  • In tri-isopropyl cation, substituents are far apart, minimizing steric interference.

  • However, adding a nucleophile would change the hybridization from sp^2 to sp^3, pushing the isopropyl groups together, resulting in steric strain (B strain).

  • This steric hindrance makes the carbocation reluctant to react, increasing its stability.

Aromatic System Formation
  • The vacant p orbital of a carbocation can participate in forming a planar (4n + 2)π electron system, where n = 0, 1, 2….

  • Cycloheptatrienyl cation is unusually stable due to being a planar 6π electron aromatic system.

Reaction of Carbocations
  • Combination with an anion: Carbocations react with negatively charged species to form stable products (e.g., addition of hydrochloric acid to ethylene yielding ethyl chloride).

  • Elimination of a proton: Carbocations can donate a proton to form an unsaturated compound.

  • Structural Stability: Decrease in energy of transition state forms carbocation. The generated carbocation by unimolecular dissociation of leaving group is resonance stabilised.

Rearrangements
  • Intermolecular alkylation by carbocation can lead to polymerization reactions.

  • 1,2-hydride shift: A 1-propyl cation rearranges to form a 2-propyl cation because the latter is more stable.

Allylic Rearrangements
  • Example:

    • S_N1 solvolysis of 3-chlorobut-1-ene.

    • Rapid nucleophilic attack occurs on C1 or C3.

Carbanions

  • Carbanions are species containing a negatively charged carbon atom.

  • The central carbon atom is sp^3 hybridized.

  • It is surrounded by three bonding pairs and one unshared pair of electrons in an sp^3 orbital, giving it a pyramidal shape.

  • Resonance-stabilized carbanions (e.g., allylic and benzylic) are sp^2 hybridized and have a trigonal planar structure.

Factors Affecting Carbanion Stability
  • The structural features responsible for carbanion stability include:

    • The amount of ‘s’ character of the carbanion carbon atom

    • Inductive electron withdrawal

    • Conjugation with an unsaturated system

    • Aromatic system formation

‘s’ Character of the Carbanion Carbon Atom
  • An electron pair in an orbital with large s character is more tightly held by the nucleus and has lower energy.

  • Carbanion stability increases with increasing ‘s’ character: sp > sp^2 > sp^3.

Inductive Electron Withdrawal
  • Groups with electron-withdrawing inductive effects (-I) stabilize carbanions by dispersing the negative charge.

  • For example, nitrogen ylides are stabilized by the -I effect of the adjacent positive nitrogen.

Conjugation with an Unsaturated System
  • Carbanions α to a double or triple bond are stabilized by delocalization of the negative charge with the π orbitals of the multiple bond.

  • Allylic, benzylic carbanions, and carbanions attached to functional groups like -NO_2, -C≡N, >C=O are stabilized by resonance.

Aromatic System Formation
  • The unshared pair of a carbanion can participate in a planar (4n + 2)π electron system, where n = 0, 1, 2….

  • Cyclopentadienyl anion is exceptionally stable due to being a 6π electron aromatic system.

Reaction of Carbanions
  • Displacement reaction: Alkylated product formed by displacement of halogen from an alkyl halide.

  • Addition to multiple bonds: Addition of Grignard's reagent to a carbonyl group.

  • Elimination reaction: Formation of alkene by alkyl halide in presence of alcoholic alkali.

  • Combination with cation

Rearrangements
  • Wittig rearrangement: Involves the formation of a carbanion stabilized by a substitution group R or R'.

  • Stevens Rearrangement: Uses a quaternary ammonium salt as the starting material.

    • The stability of the carbanion depends on the attached group, with electron-withdrawing groups (A) increasing stability.

Free Radicals

  • Homolytic cleavage of covalent bonds results in the formation of neutral species with unpaired electrons, known as free radicals.

  • Free radicals containing odd electrons on carbon atoms are called carbon radicals or simply free radicals (e.g., methyl radical (\dot{C}H_3), phenyl radical (Ph \cdot)).

  • Free radicals are classified as primary, secondary, and tertiary based on the number of carbon atoms directly attached to the carbon atom bearing the unpaired electron.

Stability of Free Radicals
  • Hyperconjugation: Free radicals are stabilized by hyperconjugation involving α-H atoms.

  • As the number of α-H atoms increases, hyperconjugation becomes more effective, and the radical becomes more stable.

  • The stability of simple alkyl radicals follows the order: tertiary (R3\dot{C}) > secondary (R2\dot{C}H) > primary (R\dot{C}H2) > methyl (\dot{C}H3).

  • Resonance: Resonance is a significant factor in stabilizing free radicals.

    • Effective delocalization of the unpaired electron with the π orbital system occurs when the carbon bearing the odd electron is α to a double bond.

    • Allyl and benzyl radicals are particularly stable due to resonance.

  • Steric Strain

    • Tertiary radicals gain stability from steric relief when a sp^2 hybridized radical is formed from a sp^3 hybridized precursor.

    • Repulsion between bulky alkyl groups is reduced by an increase in bond angles from 109.5^o to about 120^o.

Reactions of Free Radicals
  • Reactions of free radicals result in stable products (termination reactions) or lead to other radicals (propagation reactions).

  • Common termination reactions include simple combinations of similar or different radicals.

  • Another termination process is disproportionation.

  • Principal propagation reactions include:

    • Abstraction of another atom or group, usually a hydrogen atom.

    • Addition to a multiple bond: The radical formed may add to another double bond (vinyl polymerization).

    • Decomposition

    • Rearrangement

Aromaticity

  • Aromatic compounds are conjugated planar ring systems with delocalized π-electrons and alternating double and single bonds.

  • They exhibit high stability due to filled bonding molecular orbitals and greater resonance energy.

  • Aromatic compounds follow Hückel's rule: a cyclic planar conjugated species having (4n+2)π electrons (where n = 0, 1, 2, 3…) is aromatic.

  • Each carbon must be sp^2 or sp hybridized, and each atom in the ring must have an unhybridized p orbital.

  • Delocalization of π electrons over the ring lowers electronic energy and increases stability.

  • Diamagnetic ring current shifts protons outside the ring downfield and inner protons upfield in NMR spectra; such compounds are diatropic.

Features of Non-Aromatic Compounds
  • For a molecule to be non-aromatic, it must be:

    • Cyclic or acyclic

    • Lack a continuous and overlapping p-orbital system

    • Non-planar

    • Possess $4n π-electrons (where n = any integer)

  • Hückel's rule applies only to compounds with a continuous ring of overlapping p orbitals in a planar system. Cyclooctatetraene avoids π bond overlap by assuming a non-planar ‘tub-shaped’ conformation.

Features of Anti-Aromatic Compounds
  • For a molecule to be anti-aromatic, it must:

    • Be cyclic and planar

    • Have a continuous, overlapping ring of p orbitals.

    • Exhibit increased electronic energy and decreased stability upon π-electron delocalization.

    • Possess 4n π-electrons (where n = 1, 2, 3…).

  • Anti-aromatic systems exhibit a paramagnetic ring current, shifting outer protons upfield and inner protons downfield.

Types of Aromatic Compounds
  • For 2π electron systems:

    • Follow (4n+2)π electron system.

    • Aromatic if electrons are delocalized, non-aromatic if electrons are not delocalized.

  • For 4π electron systems:

    • Belong to $4nπ electron system.

    • Anti-aromatic if electrons are delocalized, non-aromatic if electrons are not delocalized.

  • For 6π electron systems:

    • Belong to (4n+2)π electron system.

    • Aromatic if electrons are delocalized, non-aromatic if electrons are not delocalized.

  • For 8π electron systems:

    • Belong to (4n)π electron system.

    • Anti-aromatic if electrons are delocalized, non-aromatic if electrons are not delocalized.

Homoaromatic Compounds
  • Conatin one or more sp^3-hybridized carbon atoms in a conjugate cyclic ring.

  • The sp^3-hybridized carbon atoms are out of the plane of the aromatic system allowing efective orbital overlapping in closed loop.

  • Homoaromatic compound involves delocalization of π- electron cloud bypassing sp^3 hybridized atom.

Quasi-Aromatic Compounds
  • Aromatic compounds where a +ve or -ve charge is part of Hückel's rule or aromaticity, with the charge present in the ring.

Stability and Energy Order
  • Stability Order: Aromatic > Homoaromatic > Non-aromatic > Anti-aromatic.

  • Energy Order: Anti-aromatic > Non-aromatic > Homoaromatic > Aromatic

Heterocycles

A heterocyclic compound is a cyclic compound that contains ring atom(s) other than carbon (N, O, S, P).

3-Membered Ring Heterocyclic Compounds
4-Membered Ring Heterocyclic Compounds
  • The Azete is an anti-aromatic compound.

  • In counting the number of π-electrons, you count the electrons which are delocalized over the ring.

  • In this case the nitrogen lone pair is localised and does not participate in resonance.

  • The nitrogen lone pair is in an sp^2 orbital which is orthogonal to the π system

  • So, the total number of π-electrons is only four: two from each double bond.

Five Membered Heterocycle: Pyrrole
  • Aromatic with 6π electrons

  • Sp^2 hybridised and planar

  • Lone pair is tied up in the aromatic ring

  • π-electron excessive; Electrophilic Aromatic Substitution is easy and Nucleophilic Substitution is difficult

Six Membered Heterocycle: Pyridine
  • Pyridine replaces the CH of benzene by a N atom (and a pair of electrons)

  • Hybridization = sp^2 with similar resonance stabilization energy

  • Lone pair of electrons not involved in aromaticity

  • Pyridine is a weak base

  • Pyridine is π-electron deficient; Electrophilic aromatic substitution is difficult and Nucleophilic aromatic substitution is easy

Fused Heterocyclic Compounds: Indole
  • Aromatic due to 10 π-electrons

  • Benzene part is non-reactive

  • Electrophilic aromatic substitution occurs at the 3- position

Organic Transformations for Making Useful Drugs

Aspirin (Acetyl Salicylic Acid)
  • Properties

    • Colourless / white crystalline solid, smells similar to vinegar.

    • Melting point of aspirin is 135 deg C, & decomposes at higher temperature.

  • Synthetic Route: The synthesis of aspirin is an esterification reaction.

    • Salicylic acid is treated with acetic anhydride, an acid derivative, causing a chemical reaction that turns OH group of salicylic acid into an ester group (R-OH → R- OCOCH3). This process yields aspirin and acetic acid. The catalyst used in this reaction is sulphuric acid or phosphoric acid.

  • Applications: Most commonly used as an anti-inflammatory and antipyretic.

Paracetamol

*Properties
* Melting point 169 °C (336 °F)

*Application
* Paracetamol is a common painkiller (analgesic) used to treat aches and pain.
* It can also be used to reduce a high temperature (antipyretic).
* Paracetamol's effects are thought to be related to inhibition of prostaglandin synthesis.

Dyes

  • Dyes are colored organic compounds used to impart color to various substances like fabrics, paper, food, hair, and drugs.

  • Dyes are soluble in water and/or an organic solvent, while pigments are insoluble in both.

Classification of Dyes
  • On the Basis of Source:

    • Natural dyes: derived from plants, invertebrates, or minerals.

    • Synthetic Dyes: Synthetic dyes are manufactured from organic molecules.

  • On the Basis of Chromophore:

  • Azo dyes: characterized by the presence of one or more azo groups —N = N—.

  • Triphenylmethane Dyes: have poor resistance to light and chemical bleaches.

  • Phthalein dyes: a class of dyes mainly used as pH indicators

Chemistry of Dyeing
  • Dyeing is applying color to fiber stock, yarn, or fabric with relatively permanent coloration.

  • Important determinants are coloration and absorption.

  • Coloration: Must be relatively permanent and not fade rapidly on exposure to light.

  • Absorption: Dye molecules concentrate on the fiber surface and are bound by:

    • Ionic forces

    • Hydrogen bonding

    • Van der Waals forces

    • Covalent chemical linkages

  • Exhaustion: In any dyeing process, heat must be supplied to the dye bath; energy is used in transferring dye molecules from the solution to the fiber as well as in swelling the fiber to render it more receptive.

  • Important Quality: evenness of dyeing, known as levelness is an important quality in the dyeing of all forms of natural and synthetic fibers.

Examples of Dyes
Methyl Orange
  • A pH indicator used in titrations.

  • Prepared from sulfanilic acid and N,N-dimethylaniline.

Indigotin
  • A distinctive blue dye known since prehistoric times, playing a key role in economies because of the rarity of natural blue dyes.

  • The chemical in indigo which is responsible for the blue colour is indigotin, which is a dark blue powder at room temperature and is insoluble in water and ethanol.